Nitrogen-doped graphene (NG) is a promising conductive matrix material for fabricating high-performance Li/S batteries. Here we report a simple, low-cost, and scalable method to prepare an additive-free nanocomposite cathode in which sulfur nanoparticles are wrapped inside the NG sheets (S@NG). We show that the Li/S@NG can deliver high specific discharge capacities at high rates, that is, ∼ 1167 mAh g(-1) at 0.2 C, ∼ 1058 mAh g(-1) at 0.5 C, ∼ 971 mAh g(-1) at 1 C, ∼ 802 mAh g(-1) at 2 C, and ∼ 606 mAh g(-1) at 5 C. The cells also demonstrate an ultralong cycle life exceeding 2000 cycles and an extremely low capacity-decay rate (0.028% per cycle), which is among the best performance demonstrated so far for Li/S cells. Furthermore, the S@NG cathode can be cycled with an excellent Coulombic efficiency of above 97% after 2000 cycles. With a high active S content (60%) in the total electrode weight, the S@NG cathode could provide a specific energy that is competitive to the state-of-the-art Li-ion cells even after 2000 cycles. The X-ray spectroscopic analysis and ab initio calculation results indicate that the excellent performance can be attributed to the well-restored C-C lattice and the unique lithium polysulfide binding capability of the N functional groups in the NG sheets. The results indicate that the S@NG nanocomposite based Li/S cells have a great potential to replace the current Li-ion batteries.
Novel sulfur (S) anchoring materials and the corresponding mechanisms for suppressing capacity fading are urgently needed to advance the performance of Li/S batteries. Here, we designed and synthesized a graphene-like oxygenated carbon nitride (OCN) host material that contains tens of micrometer scaled two-dimensional (2D) rippled sheets, micromesopores, and oxygen heteroatoms. N content can reach as high as 20.49 wt %. A sustainable approach of one-step self-supporting solid-state pyrolysis (OSSP) was developed for the low-cost and large-scale production of OCN. The urea in solid sources not only provides self-supporting atmospheres but also produces graphitic carbon nitride (g-C3N4) working as 2D layered templates. The S/OCN cathode can deliver a high specific capacity of 1407.6 mA h g(-1) at C/20 rate with 84% S utilization and retain improved reversible capacity during long-term cycles at high current density. The increasing micropores, graphitic N, ether, and carboxylic O at the large sized OCN sheet favor S utilization and trapping for polysulfides.
Traumatic brain injury (TBI) is one of the most dangerous acute diseases resulting in high morbidity and mortality. Current methods remain limited with respect to early diagnosis and real‐time feedback on the pathological process. Herein, a targeted activatable fluorescent nanoprobe (V&A@Ag2S) in the second near‐infrared window (NIR‐II) is presented for in vivo optical imaging of TBI. Initially, the fluorescence of V&A@Ag2S is turned off owing to energy transfer from Ag2S to the A1094 chromophore. Upon intravenous injection, V&A@Ag2S quickly accumulates in the inflamed vascular endothelium of TBI based on VCAM1‐mediated endocytosis, after which the nanoprobe achieves rapid recovery of the NIR‐II fluorescence of Ag2S quantum dots (QDs) owing to the bleaching of A1094 by the prodromal biomarker of TBI, peroxynitrite (ONOO−). The nanoprobe offers high specificity, rapid response, and high sensitivity toward ONOO−, providing a convenient approach for in vivo early real‐time assessment of TBI.
Most simple magnesium salts tend to passivate the Mg metal surface too quickly to function as electrolytes for Mg batteries. In the present work, an electroactive salt [Mg(THF)6 ][AlCl4 ]2 was synthesized and structurally characterized. The Mg electrolyte based on this simple mononuclear salt showed a high Mg cycling efficiency, good anodic stability (2.5 V vs. Mg), and high ionic conductivity (8.5 mS cm(-1) ). Magnesium/sulfur cells employing the as-prepared electrolyte exhibited good cycling performance over 20 cycles in the range of 0.3-2.6 V, thus indicating an electrochemically reversible conversion of S to MgS without severe passivation of the Mg metal electrode surface.
An in situ electrochemical scanning electronic microscopy method is developed to systematically study the lithium plating/stripping processes in liquid electrolytes. The results demonstrate that the lithium dendrite growth speed and mechanism is greatly affected by the additives in the ether-based electrolyte.
Fiber‐supercapacitors (FSCs) are promising energy storage devices that can complement or even replace microbatteries in miniaturized portable and wearable electronics. Currently, a major challenge for FSCs is achieving ultrahigh volumetric energy and power densities simultaneously, especially when the charge/discharge rates exceed 1 V s−1. Herein, an Au‐nanoparticle‐doped‐MnOx@CoNi‐alloy@carbon‐nanotube (Au–MnOx@CoNi@CNT) core/shell nanocomposite fiber electrode is designed, aiming to boost its charge/discharge rate by taking advantage of the superconductive CoNi alloy network and the greatly enhanced conductivity of the Au doped MnOx active materials. An all‐solid‐state coaxial asymmetric FSC (CAFSC) prototype device made by wrapping this fiber with a holey graphene paper (HGP) exhibits excellent performance at rates up to 10 V s−1, which is the highest charge rate demonstrated so far for FSCs based on pseudocapacitive materials. Furthermore, our fully packaged CAFSC delivers a volumetric energy density of ≈15.1 mW h cm−3, while simultaneously maintaining a high power density of 7.28 W cm−3 as well as a long cycle life (90% retention after 10 000 cycles). This value is the highest among all reported FSCs, even better than that of a typical 4 V/500 µA h thin‐film lithium battery.
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